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Kinetic study of key species and reactions of atmospheric pressure pulsed corona discharge in humid air

Plasma Science and Technology 2022年第5期24卷 154-168页

作者： Yongkang PENG Xiaoyue CHEN Yeqiang DENG Lei LAN Haoyu ZHAN Xuekai PEI Jiahao CHEN Yukuan YUAN Xishan WEN The School of Electrical Engineering and Automation Wuhan UniversityWuhan 430072People’s Republic of China

In this study, we examined the key particles and chemical reactions that substantially influence plasma characteristics. In summarizing the chemical reaction model for the discharge process of N_(2)–O_(2)–H_(2)O(g)mixed gases, 65 particle types and 673 chemical reactions were investigated. On this basis, a global model of atmospheric pressure humid air discharge plasma was developed, with a focus on the variation of charged particles densities and chemical reaction rates with time under the excitation of a 0–200 Td pulsed electric field. Particles with a density greater than 1% of the electron density were classified as key particles. For such particles, the top ranking generation or consumption reactions(i.e. where the sum of their rates was greater than 95% of the total rate of the generation or consumption reactions) were classified as key chemical reactions. On the basis of the key particles and reactions identified, a simplified global model was derived. A comparison of the global model with the simplified global model in terms of the model parameters, particle densities, reaction rates(with time), and calculation efficiencies demonstrated that both models can adequately identify the key particles and chemical reactions reflecting the chemical process of atmospheric pressure discharge plasma in humid air. Thus, by analyzing the key particles and chemical reaction pathways, the charge and substance transfer mechanism of atmospheric pressure pulse discharge plasma in humid air was revealed, and the mechanism underlying water vapor molecules’ influence on atmospheric pressure air discharge was elucidated.

关键词： atmospheric humid air key charged particles key chemical reactions reaction pathways

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Catalytic hydrodeoxygenation of pyrolysis bio-oil to jet fuel: A review

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Frontiers in Energy 2024年第5期18卷 550-582页

作者： Zhongyang Luo Wanchen Zhu Feiting Miao Jinsong Zhou State Key Laboratory of Clean Energy Utilization Zhejiang UniversityHangzhou 310027China

Bio-oil from biomass pyrolysis cannot directly substitute traditional fuel due to compositional *** hydrodeoxygenation(HDO)is the critical and efficient step to upgrade crude bio-oil to high-quality bio-jet fuel by lowering the oxygen content and increasing the heating ***,the hydrocracking reaction tends to reduce the liquid yield and increase the gas yield,causing carbon loss and producing hydrocarbons with a short *** obtain high-yield bio-jet fuel,the elucidation of the conversion process of biomass catalytic HDO is important in providing guidance for metal catalyst design and optimization of reaction *** the complexity of crude bio-oil,this review aimed to investigate the catalytic HDO pathways with model compounds that present typical bio-oil ***,it provided a comprehensive summary of the impact of physical and electronic structures of both noble and non-noble metals that include monometallic and bimetallic supported catalysts on regulating the conversion pathways and resulting product *** subsequent first principle calculations further corroborated reaction pathways of model compounds in atom-level on different catalyst surfaces with the experiments above and illustrated the favored C-O/C-O scission orders thermodynamically and ***,it discussed hydrogenation effects of different H-donors(such as hydrogen and methane)and catalysts deactivation for economical and industrial *** on the descriptions above and recent researches,it also elaborated on catalytic HDO of biomass and bio-oil with multi-functional ***,it presented the challenges and future prospective of biomass catalytic HDO.

关键词： biomass pyrolysis oil bio-jet fuel catalytic hydrodeoxygenation(HDO) metal catalyst reaction pathways

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Hydrogen evolution reaction between small-sized Zr_(n)(n=2–5)clusters and water based on density functional theory

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Chinese Physics B 2023年第6期32卷 429-434页

作者：唐雷雷史顺平宋永胡家宝刁凯蒋静段湛江陈德良 College of Mathematics and Physics Chengdu University of TechnologyChengdu 610059China School of Physics and Electronics Guizhou Education UniversityGuiyang 550018China

Density functional theory(DFT)is used to calculate the most stable structures of Zr_(n)(n=2-5)clusters as well as the adsorption energy values of Zr_(n)(n=2-5)clusters after adsorbing single water *** results reveal that there is a significant linear relationship between the adsorption energy values and the energy gaps of the Zr_(n)(n=2-5)***,the calculations of the reaction paths between Zr_(n)(n=2-5)and single water molecule show that water molecule can react with Zr_(n)(n=2-5)clusters to dissociate,producing hydrogen,and O atoms mix with the clusters to generate Zr_(n)O(n=2-5),all of which are exothermic *** to the released energy,the Zr4 cluster is the most efficient in Zr_(n)(n=2-5)clusters reacting with single water *** natural population analysis(NPA)and density of states(DOS)demonstrate the production of hydrogen and orbital properties in different energy ranges,respectively,jointly forecasting that Zr_(n)O(n=2-5)will probably continue to react with more water *** findings contribute to better understanding of Zr's chemical reactivity,which can conduce to the development of effective Zr-based catalysts and hydrogen-production methods.

关键词： density functional theory hydrogen evolution reaction NBO analysis reaction pathways

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Optimizing support acidity of NiMo catalysts for increasing the yield of benzene, toluene and xylene in tetralin hydrocracking

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Frontiers of Chemical Science and Engineering 2024年第1期18卷 71-84页

作者： Feng Chen Jianing Huo Liang Zhao Jinsen Gao Chunming Xu State Key Laboratory of Heavy Oil Processing China University of PetroleumBeijing 102249China

To enhance the yields of benzene,toluene,and xylene in tetralin hydrocracking,the effect of the support acid properties of NiMo catalysts on hydrocracking performance of tetralin were investigated in this *** zeolites were modified by hydrothermal treatment to form USY zeolites at different temperatures and adjust the type and amount of *** addition,H-Beta was loaded into the USY to further adjust the acidic properties of the *** result shows that when the total B acid content of the catalyst is maintained between 150 and 200μmol·g^(-1),the total acid amount is maintained between 1.7 and 1.9 mmol·g^(-1),and the L/B(L and B acids)ratio is maintained between 1.5 and 2,the catalysts have favorable performances on tetralin *** this condition,the catalysts have a yield of benzene,toluene,and xylene higher than 30 wt%and a selectivity for benzene,toluene,and xylene higher than 35%.The tetralin conversion is greater than 85 wt%.The AB6 catalyst obtains the best hydrocracking effect with the conversion of tetralin reaching 90.24 wt%,the yields of benzene,toluene,and xylene reaching 33.58 wt%,and the selectivity of benzene,toluene,and xylene reaching 37.21%,respectively.

关键词： hydrocracking tetralin benzene toluene and xylene acid properties reaction pathways

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Identification and Analysis of the Intermediates from Photodegradation of 3,3′-diamino-4,4′-azoxyfurazan(DAAF)by SERS and HPLC–MS/MS

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Journal of Analysis and Testing 2024年第3期8卷 351-360页

作者： Qi Wu Zhenqi Zhang Wenxu Zheng Juan Li Nan Ma Rui Li Bo Yang Weimiao Wang Xiaodong Li Meikun Fan Faculty of Geosciences and Environmental Engineering Southwest Jiaotong UniversityChengdu611756China Institute of Chemical Materials China Academy of Engineering PhysicsMianyang621900China College of Materials and Energy South China Agricultural UniversityGuangzhou510642China Southwest University of Science and Technology Mianyang621010China

Understanding the structural changes and degradation mechanisms of organic pollutants is critical in environmental *** this work,a xenon lamp was used as an analog light source to simulate the effect of sunlight on 3,3′-diamino-4,4′-azoxyfurazan(DAAF)in aqueous *** high-performance liquid chromatography coupled with tandem mass spectrometry(HPLC–MS/MS),surface-enhanced Raman spectroscopy(SERS)with density functional theory(DFT),the degradation intermediates and mechanisms of DAAF were *** sequential breakdown of the–NH2 and–O–N=bonds,followed by the removal of atomic O from–N=N(O)–,was emphasized and investigated using two-dimensional correlation spectroscopy(2D-COS)and SERS *** intermediates with mass-to-charge ratios(m/z)181,251 and 180 were identified and characterized by integrating experimental SERS data with DFT-calculated Raman spectra based on structures hypothesized from MS *** findings from HPLC–MS and SERS not only corroborate each other but also provide a foundation for a detailed examination of the DAAF degradation process.

关键词： DAAF Photodegradation products reaction pathways Surface-enhanced Raman spectroscopy(SERS) High-performance liquid chromatography coupled with tandem mass spectrometry(HPLC-MS/MS)

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Recent progress of electrochemical reduction of CO_(2)by single atom catalysts

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Materials Reports(Energy) 2022年第3期2卷 3-21页

作者： Tian Wang Jincheng Zhang Fuhua Li Bin Liu Sibudjing Kawi Department of Chemical&Biomolecular Engineering National University of Singapore117585Singapore School of Chemical and Biomedical Engineering Nanyang Technological University637459Singapore

Powered by electricity from renewable energies,electrochemical reduction of CO_(2)could not only efficiently alleviate the excess emission of CO_(2),but also produce many kinds of valuable chemical *** various catalysts,single atom catalysts(SACs)have attracted much attention due to their high atom utilization efficiency and expressive catalytic ***,SACs serve as an ideal platform for the investigation of complex reaction pathways and mechanisms thanks to their explicit active *** this review,the possible re-action pathways for the generation of various products(mainly C1 products for SACs)were firstly ***,recent progress of SACs for electrochemical reduction of CO_(2)was discussed in aspect of different central metal *** the most popular and efficient coordination modulation strategy,introducing heteroatom was then ***,as an extension of SACs,the development of dual atom catalysts was also briefly *** last,some issues and challenges regarding the SACs for CO_(2)reduction reaction(CO_(2)RR)were listed,followed by corresponding suggestions.

关键词： Single atom catalysts CO_(2)reduction reaction reaction pathways Coordination modulation Dual atom catalysts

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Challenges in Photocatalytic Carbon Dioxide Reduction

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Precision Chemistry 2024年第2期2卷 49-56页

作者： Guangfu Liao Guixiang Ding Bin Yang Chunxue Li National Forestry and Grassland Administration Key Laboratory of Plant Fiber Functional Materials College of Material EngineeringFujian Agriculture and Forestry UniversityFuzhou 350002China School of Chemistry and Chemical Engineering/State Key Laboratory Incubation Base for Green Processing of Chemical Engineering Shihezi UniversityShihezi 832003China College of Ecological Environment and Urban Construction Fujian University of TechnologyFuzhou 350118China

An energy crisis and significant anthropogenic CO_(2)emissions as a result of rising fossil fuel consumption have caused a rapid increase in global *** of the best solutions to these two issues is thought to be the photocatalytic reduction of CO_(2)into value-added carbon-containing *** this aspect,the main challenges mainly include the photocatalytic mechanism,reaction activity,and product selectivity,especially in ambiguous reaction pathways and product selectivity,an unclear charge transfer mechanism,and an overestimate of product ***,in this perspective,we attempt to exhibit the discussion and in-depth analysis of the possible reaction pathways and product selectivity,the specific charge transfer mechanism,and the origin of carbon-containing products in phtocatalytic CO_(2)***,the fundamentals for photocatalytic CO_(2)reduction are also ***,the state-of-the-art challenges and perspectives in CO_(2)photoreduction are highlighted and discussed in *** perspective is expected to evoke more research attention for the photocatalytic reduction of CO_(2)into value-added products.

关键词： Phtocatalytic CO_(2)reduction reaction pathways Product Selectivity Charge Transfer Mechanism Overestimate of Product Yield

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Advances and challenges of photocatalytic technology for air purification

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National Science Open 2022年第2期1卷 86-109页

作者： Qin Geng Hong Wang Ruiming Chen Lvcun Chen Kanglu Li Fan Dong Yangtze Delta Region Institute(Huzhou) University of Electronic Science and Technology of ChinaHuzhou 313000China Research Center for Environmental and Energy Catalysis Institute of Fundamental and Frontier SciencesUniversity of Electronic Science and Technology of ChinaChengdu 611731China

With the acceleration of the urban industrialization process,air pollutant emission has increased sharply,which seriously endangers the ecological environment and human ***-driven photocatalysis has the broad-spectrum activity for various inorganic to organic pollutants at ambient temperature without harsh reaction conditions,which shows a very broad application prospect in air ***,the photocatalysis technology suffers from the unrevealed reaction me-chanism and the deactivation of photocatalysts,which severely limits its practical ***,there is still a huge gap between basic research and industrial application in the field of photocatalytic air *** review summarizes recent progress on photocatalytic degradation of air pollutants and categorizes them based on the types of photocatalytic materials and air pollutants,with a focus on photocatalytic reaction mechanisms and the application scenarios of photocatalytic air purification to identify this *** also critically discussed the major challenges for promoting applications of photo-catalytic technology and put forward the development prospect.

关键词： photocatalytic technology air purification air pollutants reaction pathways application scenarios

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Methanol plasma-catalytic degradation over CeO2 catalysts: effect of ceria morphology and reaction mechanism

Methanol plasma-catalytic degradation over CeO2 catalysts: e...

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第十一届全国环境催化与环境材料学术会议

作者： Xueqing Wang Junliang Wu Jialin Wang Daiqi Ye School of Environment and Energy South China University of Technology

The effect of CeO morphology and reaction mechanism have been investigated in details on the plasma-catalytic oxidation of methanol. CeO with different morphologies(rod, particle, and cube) were prepared by a hydrothermal method and characterized by XRD, SEM, BET, Raman and XPS. The smallest particle size, the largest specific surface area and the most amount of oxygen vacancies could be achieved with CeO rod catalyst. Then all the catalysts were tested for methanol oxidation in plasma, and the results showed that CeO rod catalyst exhibited the highest removal efficiency, CO selectivity and ozone suppression. In-situ Raman spectroscopy experiments proved that the decomposition of ozone was related to the oxygen vacancy on the CeO [1]. CeO rod had the most surface oxygen vacancies, indicating that there were more active sites for ozone decomposition, and thus producing more reactive oxygen species could effectively oxidize methanol and increase CO selectivity. Compared with the oxidation of CO, the deep oxidation of methanol was the main reason why ozone improved CO selectivity in the plasma-catalytic system. Finally, the evolution of adsorbed intermediate species and some key steps of methanol oxidation were discussed based on the in-situ FTIR experiments. This work provided theoretical basis and guiding significance for improving the degradation of pollutants by optimizing the morphology of the catalyst in the plasma-catalyst system.

关键词： Plasma-catalytic CeO2 Methanol Morphology reaction pathways

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